Heterogeneous Photocatalytic Recycling of FeX2/FeX3 for Efficient Halogenation of C-H Bonds Using NaX

被引:11
|
作者
Ye, Jiani [1 ,2 ]
Zhang, Dongsheng [1 ,2 ]
Salli, Sofia [3 ]
Li, Yajiao [1 ,2 ,5 ]
Han, Feiyu [1 ]
Mai, Yuanqiang [1 ]
Rosei, Federico [1 ,4 ]
Li, Yongwang
Yang, Yong [2 ,5 ]
Besenbacher, Flemming [6 ]
Niemantsverdriet, Hans [2 ,7 ]
Richards, Emma [3 ]
Su, Ren [1 ,2 ]
机构
[1] Soochow Univ, Soochow Inst Energy & Mat Innovat SIEMIS, Suzhou 215006, Peoples R China
[2] SynCat Beijing Synfuels China Technol Co Ltd, SynCat Beijing, Leyuan South St 2,1 Yanqi Econ Dev Zone C, Beijing 101407, Peoples R China
[3] Cardiff Univ, Sch Chem, Pk Pl, Cardiff CF10 3AT, Wales
[4] Inst Natl Rech Sci, Ctr Energy Mat & Telecommun, 1650 Blvd Lionel Boulet, Varennes, PQ J3X 1P7, Canada
[5] Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
[6] Aarhus Univ, Interdisciplinary Nanosci Ctr, Gustav Wieds Vej 14, DK-8000 Aarhus, Denmark
[7] SynCat DIFFER Syngaschem BV, NL-6336 HH Eindhoven, Netherlands
基金
英国工程与自然科学研究理事会;
关键词
Flow Synthesis; Green Chemistry; Halogenation; Heterogeneous Photocatalysis; Oxidant Free; VISIBLE-LIGHT; OXIDATIVE CHLORINATION; BROMINATION; CATALYST; HYDROCARBONS; CYCLOHEXANE; GENERATION; HALIDES; ARENES;
D O I
10.1002/anie.202302994
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Environmental-friendly halogenation of C-H bonds using abundant, non-toxic halogen salts is in high demand in various chemical industries, yet the efficiency and selectivity of laboratory available protocols are far behind the conventional photolytic halogenation process which uses hazardous halogen sources. Here we report an FeX2 (X=Br, Cl) coupled semiconductor system for efficient, selective, and continuous photocatalytic halogenation using NaX as halogen source under mild conditions. Herein, FeX2 catalyzes the reduction of molecular oxygen and the consumption of generated oxygen radicals, thus boosting the generation of halogen radicals and elemental halogen for direct halogenation and indirect halogenation via the formation of FeX3. Recycling of FeX2 and FeX3 during the photocatalytic process enables the halogenation of a wide range of hydrocarbons in a continuous flow, rendering it a promising method for applications.
引用
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页数:7
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